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Activating lattice oxygen of two-dimensional MnXn-1O2 MXenes via zero-dimensional graphene quantum dots for water oxidation

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Science China Materials 2022年第11期65卷 3053-3061页

作者： Yiyuan Ma Yurong An Zhuo Xu Laifei Cheng Wenyu Yuan Science and Technology on Thermostructural Composite Materials Laboratory School of Materials Science and EngineeringNorthwestern Polytechnical UniversityXi’an 710072China State Key Laboratory of Solidification Processing School of Material Science and EngineeringNorthwestern Polytechnical UniversityXi’an 710072China Shaanxi Key Laboratory for Advanced Energy Devices Shaanxi Engineering Lab for Advanced Energy TechnologyInstitute for Advanced Energy MaterialsSchool of Materials Science and EngineeringShaanxi Normal UniversityXi’an 710119China Key Laboratory of Macromolecular Science of Shaanxi Province Key Laboratory of Applied Surface and Colloid ChemistrySchool of Chemistry&Chemical EngineeringShaanxi Normal UniversityXi’an 710062China

The poor oxygen evolution reaction(OER)activity of two-dimensional(2 D)transition metal carbides(MXenes)is a major obstacle to their application in highperformance water splitting and fuel cells due to the high energy barriers for the absorption of ***,we demonstrate that the lattice oxygen of M_(n)X_(n-1)O_(2)MXenes can be activated by 0 D graphene quantum dots(GQDs),thereby activating the OER via the lattice-oxygen oxidation mechanism(LOM)instead of the conventional adsorbate evolving *** pH-dependent OER activity of M_(n)X_(n-1)O_(2)@GQDs and ^(18)O isotope-labelling experiments with time-of-flight secondary-ion mass spectrometry(TOF-SIMS)provide the direct evidence of ***,the activated lattice oxygen amount can be controlled by the *** as-prepared 0 D/2 D Ti_(3)C_(2)O_(2)@GQDs heterostructure delivers a highly reduced overpotential of 390 mV(bare Ti_(3)C_(2)O_(2):530 mV)at a benchmark current density of 10 mA cm^(-2).Through optimizing the thickness and the additional conductive substrate,the overpotential at 10 mA cm^(-2)decreases to 250 mV,while the Tafel slope is reduced to 39 mV dec^(-1);these values indicate the as-prepared heterostructure is superior to the state-of-the-art MXene-based OER *** work provides a new strategy to enhance the OER activity of M_(n)X_(n-1)O_(2)and extends the application of LOM from perovskite to MXenes.

关键词： graphene quantum dots lattice-oxygen activation oxygen evolution reaction water splitting heterostructure

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